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Fuel Processing Technology 91 (2010) 16171623

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Fuel Processing Technology


j o u r n a l h o m e p a g e : w w w. e l s ev i e r. c o m / l o c a t e / f u p r o c

Oxy-fuel circulating uidized bed combustion in a small pilot-scale test rig


T. Czakiert a,, K. Sztekler a,b, S. Karski a, D. Markiewicz a,b, W. Nowak a
a b

Czestochowa University of Technology, Faculty of Environmental Protection and Engineering, Dabrowskiego 73, 42-200 Czestochowa, Poland Foster Wheeler Energia Polska Sp. z o.o., Staszica 31, 41-200 Sosnowiec, Poland

a r t i c l e

i n f o

a b s t r a c t
Coal combustion under the elevated partial pressure of oxygen in a circulating uidized bed environment was investigated. The fuel used was bituminous coal. The concentration of oxygen in the air was increased to 35% per volume. Excess oxygen ranged from 1.1 to 1.3 and the temperature ranged from ca. 1073 K to 1273 K. A 0.1 MWth CFB combustor was adapted for oxy-combustion. The conversion ratios respectively studied were: carbon, sulfur and nitrogen to CO, SO2 and NOX. An increase of nitrogen and sulfur conversion ratios and a strong decrease of incomplete combustion losses were found under the oxygen-enriched conditions. Moreover, a strong increase in temperature was noticed during oxy-combustion. 2010 Elsevier B.V. All rights reserved.

Article history: Received 3 December 2009 Received in revised form 20 June 2010 Accepted 22 June 2010 Keywords: Oxy-combustion CFB Coal Pilot-scale

1. Introduction Oxy-fuel combustion is a response to the need to reduce CO2 emission from the largest point source, power generation. It results from highly concentrated CO2 stream obtained from oxy-combustion, which can be directly sequestrated [1]. Further advantages of high fuel exibility and operating exibility [2] appear when oxycombustion is introduced into a circulating uidized bed (CFB) environment. However, the main benet of CFB is the reduction in the amount of returned ue gas, which results from the circulating solids used for cooling [3]. A major milestone in the development of oxy-fuel combustion technology seems to be reached in 2008, when Vattenfall and Alstom successfully completed the commissioning the world's rst full chain 30 MWth Oxy-Fuel PC Pilot Plant Facility with CO2 Capture located in Schwarze Pumpe, Germany [4]. Work on a 500 MWth OxyFuel PC Demonstration Plant is currently in progress [5]. Oxy-fuel CFB technology remains much less developed. Work in this eld has been conducted by: Foster Wheeler Energia Oy [6], VTT [7] and CANMET [8]. Interesting results from a 0.3 MWth CFB Pilot-Scale Test Facility are also reported by Eddings et al. [9]. The comprehensive review of the latest evaluation of oxy-fuel combustion technology in circulating uidized bed is given by Zhao et al. [10], while Kanniche et al. [11] compare the economics of oxy-combustion with other CO2-free power generation technologies. Implication of oxy-fuel combustion in supercritical steam boilers is studied by Horbaniuc

et al. [12]. Nevertheless, the gap between the development of oxy-PC and oxy-CFB technologies remains signicant. Therefore, the paper presents author's rst experience from a 0.1 MWth Oxy-Fuel CFB test rig.

2. Experimental The investigations were carried out on a 0.1 MWth CFB test rig modied for oxy-combustion (Fig. 1). The unit consists of a 0.1 m I.D., approximately 5.0 m tall combustion chamber, connected via a crossover section to a 0.25 m I.D. hot cyclone. Solids separated in the cyclone return to the combustion chamber via a 0.075 m I.D. downcomer and a nonmechanical loopseal. The unit is provided with four heaters, three around the combustion chamber and one around the downcomer. These furnaces are used to heat the unit to (or beyond) the ignition point of the fuel being used. Fluidizing oxygen-enriched air (PA) is supplied through a common-rail tted with four nozzles at the bottom of the combustion chamber. This gas may be preheated with the help of two heaters installed in series. Secondary air (SA) may be provided optionally at three levels of the combustion chamber. The oxygen fractions in PA and SA may be different due to two independent ow mixers. Fuel is fed continuously by a screw feeder above the primary air nozzles. A single fabric lter baghouse, installed downstream of the cyclone, is used for ultimate ue gas particulate clean-up. The baghouse may be by-passed if necessary. Flue gas leaving the baghouse (or by-passing the baghouse) is vented with the help of an ID fan to the atmosphere, through a stack. The test rig is equipped with developed data acquisition system for temperature (T) and pressure (P or DP) measurements as well as a

Corresponding author. Tel.: +48 34 3250945; fax: +48 34 3250933. E-mail address: tczakiert@is.pcz.czest.pl (T. Czakiert). 0378-3820/$ see front matter 2010 Elsevier B.V. All rights reserved. doi:10.1016/j.fuproc.2010.06.010

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T. Czakiert et al. / Fuel Processing Technology 91 (2010) 16171623

Fig. 1. 0.1 MWth Oxy-Fuel CFB test rig.

number of ports for ue gas (FG), bottom ash (BA), y ash (FA) and circulating material (CM) sampling. Round sand of ca. 250630 10 6 m in size and d3,2 = 400 10 6 m (see: Fig. 2) was used as initial bed material. Total mass of circulating solids was mbm = 8 kg. The minimum uidizing velocity (umf) [13] and the terminal velocity (ut) [13] calculated for the coarsest particles and the investigated conditions were 0.13 m s 1 and 5.0 m s 1, respectively. Oxygen concentration in the air was increased to 35% per volume and excess oxygen ranged from 1.1 to 1.3. For the tests, bituminous coal was selected. Properties of the fuel are given in Table 1 and Table 2 whereas the distribution of particles size ranged from ca. 100 10 6 to 2500 10 6 m (d3,2 = 450 10 6 m) is shown in Fig. 2. The temperature ranged from ca. 1073 K to 1273 K. Sampling frequency for temperature and pressure was 1 Hz. Infrared (CO2, CO, SO2, and NOX) and

paramagnetic (O2) methods of measurement for the foregoing ue gas components were employed. Measurement time was established at 600 s and starts after stable operating conditions in the combustor are achieved. Conversion ratios (CR) of the following fuel constituents, i.e. combustible sulfur (Scomb fuel ), molecular nitrogen (Nfuel) and carbon (Cfuel) to SO2, NOX and CO, respectively, were used to study of fuel behavior during oxy-combustion in CFB environment. It was assumed that: (i) the distribution of C, S and N within volatile matter as well as char is uniform, which can be only valid if the amount of unburned char is very small; (ii) carbon conversion ratio to CO2 + CO corresponds to burn-out ratio of combustible matter of fuel; (iii) airnitrogen does not convert to NOX under the investigated conditions, which can be only valid if the temperature of ca. 1500 C is not exceeded. Thus, the values

T. Czakiert et al. / Fuel Processing Technology 91 (2010) 16171623 Table 2 Composition of fuel-ash (XRF analysis). Element Al Si P S Cl K Ca Ti V Cr Mn Fe Co Ni Cu Zn Sn Sb Pb Naa Mga
a

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Fraction (wt.%) 5.0 9.4 0.5 b 0.14 0.53 0.02 0.087 0.015 1.47 0.07 0.61 0.03 0.244 0.007 0.0047 0.0007 0.013 0.001 0.0266 0.0014 1.76 0.075 0.0139 0.0013 0.0025 0.0003 0.0011 0.0002 0.0135 0.0006 b 0.00045 b 0.0005 0.0074 0.0003 0.54 0.03 0.53 0.03

Fig. 2. Particle size distribution for sand and fuel.

of CRS N SO2, CRN N NOx and CRC N CO can be calculated using following equations (Eqs. ((1)(7))): conversion ratio of combustible sulfur contained in fuel to SO2: Sfg CRSNSO2 =
SO2

AAS analysis.

CO2CO Cfg

and, molar ratio of N2/C in fuel: 1 N kmol  Nfuel N2 = 28 C C fuel kmolC 12 6

Scomb fuel C fuel

where:molar ratio of S (xed in SO2)/C (xed in CO2 + CO) in ue gas:


2 SSO fg CO2CO Cfg

  SO2 kmolS 10 CO2 + CO kmolC


4

conversion ratio of carbon contained in fuel to CO, which is directly expressed as molar ratio of C (xed in CO)/C (xed in CO2 + CO) in ue gas: CRC N =
CO Cfg CO2 + CO Cfg

CO

and, molar ratio of combustible S/C in fuel: S kmol  Scomb S fuel = 32 C kmol C fuel C 12

CO : 104 CO2 + CO

conversion ratio of molecular nitrogen contained in fuel to NOX: Nfg


NOx

The main advantage of this manner of analyses is the independence of the results from: (i) changes in the moisture and ash contents in the fuel; (ii) changes in the volatileschar ratio; (iii) values of the incomplete combustion losses; and (iv) measurements of fuel ux as well as air and oxygen uxes; which is helpful during pilot-scale investigations. 3. Results and discussion Initially, air-ring experiments were performed to provide a background for oxy-combustion tests. Changes in temperature and pressure distributions along the height of combustion chamber were analyzed in a broad range of investigated conditions. The distributions of solids concentration in the furnace determined for different supercial gas velocities (v= 3.65 m s 1, 4.25 m s 1 and 4.85 m s 1) are shown in Fig. 3, whereas, an example of pressure uctuations is given in Fig. 4. More uniform distribution of bed material inside the combustion chamber (see: Fig. 3) can be found for higher gas velocity. It results from declining solids concentration in the grid zone as well as from increasing concentration of bed material in the upper part of the furnace. Moreover, total pressure drop in combustion chamber is lower in case of higher gas velocity, since more coarser particles are moved to the return leg. Furthermore, the strongest pressure uctuations were recorded in the dense phase just above the grid and the lightest uctuations of pressure were measured in the upper part of the furnace with a dilute phase of solids (see: Fig. 4). All further oxy-combustion tests were conducted at the supercial gas velocity of ca. 4.80 m s 1.

CRN N NOx =

2CO C CO fg N fuel C fuel

where:molar ratio of N2 (xed in NOX)/C (xed in CO2 + CO) in ue gas: NNOx fg


CO2 + CO Cfg

  0:5NOX kmolN2 104 CO2 + CO kmolC

Table 1 Properties of bituminous coal. LHV (kJ kg 1) Proximate analysis (wt.%) 21,055 6.8 27.5 43.5 22.2 57.8 1.28 3.54 0.69 7.69

Ultimate analysis (wt.%)

Moisture VM FCby diff. Ash C S H N Oby diff.

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Fig. 3. Pressure distributions in combustion chamber of CFB test rig.

Fig. 5. Temperature proles in combustion chamber of CFB test rig.

Temperature measurements were taken at ve levels of the combustion chamber, where the mean values were a basis to establish the temperature proles shown in Fig. 5. A strong increase in temperature associated with elevated partial pressure of oxygen can be noticed, especially when the oxygen concentration is raised from 21% up to 28 vol.%. It results mainly from higher load of the combustion chamber, since the value of excess oxygen was maintained. Moreover, a decrease in temperature at the level of 3.23 m can be observed. It comes from lighter thermal insulation in the upper part of the test rig, and hence the enhanced heat-transfer, which simulates the operation of so-called Wing-Walls heat exchangers located in that part of commercial CFB boilers [14]. The comparison of average temperatures in combustion chamber estimated for different oxygen concentrations and different values of excess oxygen is presented in Fig. 6. Conversion ratios of fuel-N2 to NOX = NO + NO2 (CRN N NOx) under air-ring and oxygen-enriched conditions are shown in Figs. 7 and 8, respectively. What was found for air environment is higher values of CRN N NOx associated with both: an increase of temperature regardless of excess oxygen ( = 1.11.3) and an increase of excess oxygen in the reaction zone at stable temperature. It can be seen, for instance, the increase of nitrogen conversion ratio of more than 50% when excess oxygen is changed from 1.2 to 1.3 at T = 1074 K (see the arrow in Fig. 7). The above-mentioned fundamental relations noticed in the pilot-scale CFB test rig have been also reported from laboratory-scale experiments [15] as well as from industrial-scale investigations [16].

Further increase in conversion ratio of fuel-N2 to NOX can be observed during oxy-combustion (Fig. 8), which does not conrm the results obtained on a small laboratory-scale CFB facility [17]. However, the effect of elevated partial pressure of oxygen overlaps here the thermal effect (see also: Fig. 5). On the other hand, the nitrogen conversion ratio increases with an increase of excess oxygen in spite of decline in the temperature (see also: Fig. 6). Therefore, it can be claimed that oxygen is the crucial factor in NOX formation in CFB environment. The effect of oxygen concentration on volatiles-N conversion is deeply studied by Chaiklangmuang et al. [18]. The charN conversion (and hence overall conversion) is not considered in this case, since the process involves steps for the formation of NO and its destruction by char and thus is difcult to estimate. The results given in [18] are very close to the results presented in Fig. 8, which shows direct increase of nitrogen conversion ratio associated with the increase in O2 concentration. Nevertheless, the values of CRN N NOx remain below the level of 20% in the whole range of investigated conditions. All tests at oxygen concentration of 35% and excess oxygen of 1.1 were left out due to a strong increase in the temperature (see also: Fig. 6); it was necessary to avoid overheating the main parts of the test rig. Otherwise, conversion ratios of combustible sulfur to SO2 (CRS N SO2) are relatively high and exceed the level of 85% regardless of combustion atmosphere (Figs. 910). Generally, two main relations were found for air-ring conditions (Fig. 9). Firstly, a lower sulfur conversion ratio associated with an increase in temperature can be seen regardless of excess oxygen. It is suspected that the effect follows from bonding of S with Ca and Mg both contained in fuel-ash (see also: Table 2). Similar

Fig. 4. Pressure uctuations in combustion chamber of CFB test rig.

Fig. 6. Average temperatures in combustion chamber of CFB test rig.

T. Czakiert et al. / Fuel Processing Technology 91 (2010) 16171623

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Fig. 7. Fuel-N2 conversion ratioair-ring.

Fig. 9. Combustible sulfur conversion ratioair-ring.

behavior between sulfur and fuel-ash components in the CFB environment is also reported by Eddings et al. [9]. Moreover, a decline of sulfur conversion ratio with an increase in excess oxygen at stable temperature is noticed, which probably results from oxidation of sulfur directly to SO3. However, it can be believed that other phenomenon overlaps here this behavior due to relatively big differences between the results. Lower values of CRS N SO2 that correspond to higher excess oxygen can be also observed for oxy-combustion (Fig. 10). Similar phenomenon is found by Hack et al. [19], who analyze the effect of low excess O2 during oxy-combustion. Authors claim that formation of SO3 can be reduced by 30% due to a reduction of oxygen concentration in furnace exit gas from 3% to 1 vol.%. The reduction in the amount of SO3 (which is a very corrosive) seems to be additional benet of oxy-combustion, where excess O2 can be limited due to the elevated partial pressure of oxygen. According to Toftegaard et al. [20], it should be possible to reduce the required oxygen excess during oxy-fuel combustion to no more than 10%. Unfortunately, SO3 component was not detected in ue gas during the measuring campaign. Previous experience in the eld of oxy-fuel CFB combustion [17] indicates that higher sulfur conversion ratios (even up to 100%) can be expected, which was conrmed during the pilot-scale investigations. It results probably from the oxidation of S xed in one of the ue gas components, e.g. H2S, to SO2. In one case, however, the value of CRS N SO2 exceeds the maximum level of 100%. Because of the manner of calculation of CRS N SO2 (1), it has to follow from a slight temporary variation in the molar ratio of combustible sulfur-to-carbon in the fuel (3).

Fig. 10. Combustible sulfur conversion ratiooxy-combustion.

Similar results to those in Fig. 9 can be found for conversion of carbon to CO in air-ring conditions (Fig. 11), where CRC N CO decreases with both: an increase in temperature regardless of excess oxygen and an increase in excess oxygen at stable temperature (see the arrow in Fig. 11). Moreover, a kind of minimum level of CRC N CO seems to be established at ca. 0.2%, which does not intend to be exceeded even in case of the highest temperature (1104 K) or the highest excess oxygen (1.3). However, as can be seen in Fig. 12, a

Fig. 8. Fuel-N2 conversion ratiooxy-combustion.

Fig. 11. Carbon conversion ratioair-ring.

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Fig. 12. Carbon conversion ratiooxy-combustion.

further strong decrease of incomplete combustion losses can be achieved when oxygen concentration in gaseous environment is raised up. Nevertheless, the effect of temperature that associates with oxy-combustion (see also: Fig. 5) should be taken also into consideration. The studies on pollutant emissions from a quite similar 100 kW pilot-scale oxy-fuel circulating uidized bed combustor were recently published by Jia et al. [21]. The results obtained by Authors are very promising as well, where CO emissions during oxy-fuel CFB combustion are lower or comparable to those of air-ring. Similar conclusion was drawn from investigations conducted on 0.3 MW pilot-scale combustor, where increasing the oxygen concentration decreased the CO emission [22]. 4. Conclusions The results from the investigations conducted on a small pilotscale 0.1 MWth Oxy-Fuel CFB test rig were discussed. The effect of the elevated partial pressure of oxygen on bituminous coal combustion in a circulating uidized bed environment was analyzed under different operating conditions. Conversion ratios of sulfur, nitrogen and carbon all contained in fuel to SO2, NOX and CO, respectively, were used to compare the results obtained for air-ring and oxy-combustion. A strong increase in temperature associated with elevated partial pressure of oxygen was noticed, especially when the oxygen concentration is raised from 21% up to 28% per volume. It results mainly from the increased load of combustion chamber, since the value of excess oxygen was maintained. The values of nitrogen conversion ratio remain below the level of 20% in the whole range of investigated conditions. Higher conversion ratios of fuel-N2 to NOX associated with elevated partial pressure of oxygen as well as with an increase of excess oxygen in reaction zone were found, which proves that oxygen is the crucial factor in NOX formation in a CFB environment. Furthermore, the strong effect of temperature under air-ring conditions was also observed. Otherwise, sulfur conversion ratios are relatively high and exceed the level of 85% regardless of gaseous atmosphere. Higher conversion ratios of combustible sulfur to SO2 during oxy-combustion were noticed, which probably follows from oxidation of S xed in one of the ue gas components, e.g. H2S, to SO2. Moreover, a decline of sulfur conversion ratio with an increase in excess oxygen was observed, which probably results from the oxidation of sulfur directly to SO3. With air-ring conditions, a lower sulfur conversion ratio associated with an increase of temperature was found, also. It is suspected that the effect follows from bonding of S with Ca and Mg both contained in fuel-ash. The values of incomplete combustion losses during oxy-combustion were much below the level achieved under air-ring conditions.

Nomenclature Cfuel carbon contained in fuel, kmol CCO carbon xed in CO in ue gas, kmol fg + CO CCO2 carbon xed in CO2 + CO in ue gas, kmol fg CR conversion ratio, d3,2 Sauter diameter, m H height of combustion chamber, m mbm total mass of bed material, kg Nfuel molecular nitrogen contained in fuel, kmol NNOx molecular nitrogen xed in NOX in ue gas, kmol fg p pressure, Pa Scomb combustible sulfur contained in fuel, kmol fuel SSO2 sulfur xed in SO2 in ue gas, kmol fg t time, s T temperature, K umf minimum uidizing velocity, m s 1 ut terminal velocity, m s 1 v supercial gas velocity, m s 1 [CO] CO concentration in ue gas, ppm [CO2] CO2 concentration in ue gas, % [NOX] NOX concentration in ue gas, ppm [SO2] SO2 concentration in ue gas, ppm difference, sphericity of particles, excess oxygen, mf voidage of bed at minimum uidizing conditions, density, kg m 3

Acknowledgements Financial support of this work by the Polish Government, as a part of the Framework Project: Supercritical Coal-red Power Units, is gratefully acknowledged. References
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